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Zn-doped tubular graphene nitride for visible light and sacrificial-agent-free H2O2 photosynthesis in water
Graphitic carbon nitride (g-C 3 N 4 ) has become a favored universal photocatalyst. Despite its numerous advantages, the photocatalytic efficiency of g-C 3 N 4 is hindered by the substantial recombination of photoexcited charge carriers and holes. In this work, we demonstrate that Zn-doped tubular carbon nitride photocatalyst (Zn-tCN) can serve as highly efficient catalysts for H 2 O 2 photosynthesis. Mechanism studies confirm that the presence of Zn in g-C 3 N 4 prolongs the lifetimes of photogenerated carriers and inhibits their recombination, which triggers the reduction of O 2 to reaction intermediates ( O 2 − ), as supported by in situ electron paramagnetic resonance (EPR) spectroscopy. More importantly, sacrificial agent experiments coupled with in situ EPR results confirmed that the reaction mechanism involves a concerted two-electron transfer process. The optimal catalyst displays a H 2 O 2 productivity of 162.4μmol g –1 h −1 under visible-light irradiation without a sacrificial agent, which is 11.7 times higher than that of pristine g-C 3 N 4 (13.8μmol g –1 h −1 ). This work proposes a synthetic strategy for the preparation of high-performance Zn-doped g-C 3 N 4 , which offers insights and perspectives for developing highly active photocatalysts and deepening the understanding of photocatalytic mechanisms.